CN114424058B - Tracing method for VOCs pollution - Google Patents
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Abstract
A tracing method for VOCs pollution belongs to the field of environmental monitoring. Comprises the following steps: establishing a known source spectrum database (Si); monitoring a plurality of groups of atmospheric VOCs data; screening a known source spectrum database; modifying and converting the screened source spectrum database (Sj) to obtain a modified source spectrum database (Sj'); analyzing by using a PMF method; carrying out component characteristic comparison and correlation comparison on the pollution source component spectrum (F) and each source spectrum data in the corrected source spectrum database (Sj'); and then the contribution proportion of each known pollution source discharge port in the known source spectrum database at the monitoring point is obtained.
Description
Technical Field
The invention relates to a tracing method for VOCs pollution, belonging to the field of environmental monitoring.
Background
Volatile Organic Compounds (VOCs) are a class of important atmospheric pollutants that can be harmful to the environment or human body in different ways. Due to development and utilization of petroleum and coal and wide use of various chemicals in various industries, most of VOCs are discharged into the atmosphere, so that the VOCs are required to be identified and analyzed, and the source of the VOCs is traced, so that the discharge of the VOCs is controlled from a pollution source.
In the existing VOCs pollution source identification method, mass spectrum data acquired by fixed monitoring points are taken as reference, mass spectrum cross-correlation calibration is carried out on a plurality of currently acquired pollution source mass spectrum data, namely the types of pollution sources and the contribution rates of various pollution sources are determined according to the similarity between the acquired pollution source mass spectrum data and the mass spectrum data of the fixed monitoring points.
However, the currently adopted method for identifying the pollution sources of the VOCs needs complete mass spectrum data of the pollution sources in the identification process, the identification accuracy depends on the integrity of the mass spectrum data of the pollution sources, and the identification effect is poor.
At present, a VOCs (volatile organic compounds) pollution source positioning device collects volatile organic compounds in atmosphere of a fixed monitoring point through an atmosphere sampler, analyzes the obtained data by using a volatile organic compound mass spectrometer, obtains mass spectrum data, determines the type of a pollution source and further determines the area where the volatile organic compound pollution source is located.
The source resolving techniques that can be used mainly for tracing the sources of atmospheric VOCs are mainly classified into Emission Inventory (Emission Inventory), diffusion Model (Diffusion Model) and Receptor Model (Receptor Model).
The emission list is a list model established by observing and simulating source emission amount of the atmospheric VOCs, emission geographical distribution, emission characteristics and the like. The method for analyzing the pollution physical diffusion needs a detailed source emission list, the solving process is complex, and different emission parameters are set to greatly influence the result.
The diffusion model is a technology for estimating the contribution value of the pollution source by simulating the space-time distribution conditions of pollutants under different conditions such as emission, migration, diffusion and chemical conversion of the pollution source on the basis of having a detailed list of the pollution source and the emission amount of the pollution source. The diffusion model can well establish the quantitative relation between organized emission sources and the quality of the atmospheric environment, but cannot be applied to unorganized open sources with difficult source strength determination, and the parameters required by the model are complex (for example, the number and the orientation of pollution sources and detailed meteorological data in the diffusion process of VOCs need to be known). These data are difficult to obtain, limiting the use of the model.
The current receptor model refers to a series of source analysis technologies for determining the contribution value of various pollution sources to the receptor through chemical analysis of atmospheric VOCs and source samples. Unlike the diffusion model, the receptor model targets a contaminated area, and the use of the receptor model for source analysis does not take into account the migration process of the contaminants, the discharge conditions of the contaminants, the meteorological conditions during discharge, and the like. After sampling and analyzing, the VOCs are usually judged by adopting a receptor model to judge main pollution sources and relative contributions of various pollution sources to atmospheric pollution, but the proportion of each component in source spectrum data cannot be directly used for reflecting the proportion of each component after the source spectrum is transmitted to a monitoring point, and the influence is larger along with the increase of the distance. The data of the polluted source spectrum position is only made to correspond to the data of the monitoring point, and the problems of inaccurate source tracing and low positioning accuracy exist in the source tracing.
Disclosure of Invention
Related concepts and terms
Chemical mass balance model method (CMB): the principle of the chemical mass balance model is mass conservation, the idea is to calculate the contribution of each emission source to the receptor by using a least square method according to the detection value of the environmental receptor sample and the emission condition of each pollution emission source, and the meaning of the linear equation system is that the concentration of each receptor can be regarded as the linear sum of the products of the concentration value of each pollution source and the contribution value thereof. The input file for the model includes source composition spectral data, total mass concentration of receptors, and total mass concentration uncertainty of receptors, and the output file includes contribution values for each chemical component in each source. The uncertainty of the input file can be used not only to measure the importance of the input data in the final result, but also to calculate the uncertainty of the source contribution. The method is an important method for source analysis due to the advantages of simple principle, easiness in understanding, accurate analysis result and the like, and has the defect that a detailed source sample and receptor sample emission list is required.
Let the concentration of chemical component i contained in the acceptor be, by conservation of mass:
C i ＝∑S j ×F ij
the allocation rate of the source class j is:
η i ＝S j /C i ×100％
C i : measurement of the Mass concentration of chemical component i in the Acceptor atmosphere, μ g/m 3 ；
F ij : mass fraction measurement of chemical component i in a jth source,%;
S j : calculated mass concentration of the contribution of the j-th source, μ g/m 3 ；
i, j: number of chemical components and source classes respectively
Input quantity is F ij The output quantity is S j 、η i According to the matrix algorithm, the equation set has positive solution only when i is larger than or equal to j. Principal Component Analysis (PCA): the PCA method is a method of converting a plurality of indices into a few linearly independent synthetic indices. Principal component analysisThe basic idea of the method is that the specific gravity of each index is determined by integrating and simplifying high-dimensional variables on the basis of original data, and the method has certain objective superiority and is increasingly applied to the field of environment.
The calculation is performed by the method of calculating the number of principal components in the principal component analysis.
(1) Firstly, a correlation coefficient matrix is calculated
r ij (i, j =1,2, \8230;, p) is the original variable x i And x j Of correlation coefficient r ij ＝r ji The calculation formula is
(2) Computing eigenvalues and eigenvectors
Solving the eigen equation | λ I-R | =0, finding the eigenvalues by the Jacobi method (Jacobi) and arranging λ in order of magnitude 1 ≥λ 2 ≥…≥λ p ≥0；
(3) Calculating principal component contribution rate and accumulated contribution rate (not calculating, only for reference of number of emission sources screened later)
Contribution rate:
cumulative contribution rate:
generally, a characteristic value, lambda, with the accumulated contribution rate of 85% -95% is taken 1 ，λ 2 ，…，λ m Corresponding main components 1,2, 8230, m (m is less than or equal to p).
(4) Calculating principal component loadings
Orthogonal matrix factor analysis (PMF): the PMF method is an effective data analysis method developed on the basis of a factor analysis method, and is now widely used in the field of source analysis. The method is mainly characterized in that firstly, the weight is used for calculating the error of each species of the VOCs in the atmosphere, and then the main pollution source and the contribution rate of the VOCs are determined by the least square conjugate gradient method.
The matrix form data expression is as follows:
X＝GF+E
in the formula:
x: n multiplied by m matrix, wherein n represents the number of environmental receptor samples, and m represents the number of chemical elements in the environmental receptor;
g: an n x p emission source contribution matrix;
f: a p × m pollution source spectral composition spectral matrix;
p: the number of factors;
e: a residual matrix representing the difference between X and GF.
The objective of the PMF analysis is to minimize Q, which is defined as:
I＝1，2，.......，n；j＝1，2，……，p；k＝1，2，……，m。
in the formula: x is a radical of a fluorine atom ij 、g ij 、f ij 、e ij The elements of the X, G, F and E matrices, respectively.
At g ik ≥0，f kj Under the constraint condition of being more than or equal to 0, the method solves Q through an iterative minimization algorithm, and can simultaneously determine a pollution source contribution value G (relative value) and a pollution source composition spectrum F (relative concentration value of chemical components).
The PMF model has advantages and disadvantages, and the method has the advantages that source component spectrum data does not need to be measured, elements in a decomposition matrix are non-negative values, the optimization can be carried out by using the standard deviation of data, missing data, inaccurate data and the like can be processed. The disadvantage is that the model does not provide a method for determining the number of factors p, and the selection of the number of factors has an influence on the source resolution result.
Si: a source of pollution component spectrum;
si': correcting the component spectrum of the pollution source;
loss calculation formula of VOCs active species:
VOCs will have certain loss under atmospheric environment, convert VOCs's observation data into initial concentration data with following formula:
[voc i ] o ＝[VOC i ] t /exp(-k i [OH]Δt)
[VOC i ] o ：VOC i observations of volume fraction/values at monitoring points;
[VOC i ] t ：VOC i an initial value of volume fraction;
b, C: primary hydrocarbons HCB and HCC exhausted from the same pollution source;
k i ：VOC i 0H radical reaction rate constant;
k B : 0H radical reaction rate constant for HCB;
k C : 0H radical reaction rate constant of HCC;
[ OH ]: volume fraction of OH radicals;
Δ t: reaction time;
In determining B and C, it is preferred that B and C have homology and exhibit significant photochemical aging phenomena, such as a significant diurnal variation profile and a significant diurnal concentration reduction.
The main technical scheme is as follows:
the invention provides a tracing method for VOCs pollution, which compares the data analysis result of the pollutant components of a monitoring point with the data (or corrected source spectrum) of a known pollution source discharge port, and fully considers the influence of diffusion and photochemical reaction on the pollution source after being transmitted from the discharge port to the monitoring point, thereby improving the accuracy and reliability of the source analysis result.
Scheme 1:
the required work is to establish a known source spectrum database (Si), wherein the known source spectrum database contains information including pollutant composition proportion of a pollutant source discharge port and corresponding geographical position information; analyzing the wind speed and the wind direction at the source tracing moment, the position information of the monitoring points and the position information of the source spectrum database, and screening a discharge port of a pollution source which has great influence on the monitoring points; and converting the screened pollution source spectrum into a corrected source spectrum (Si') of the pollution source spectrum at the monitoring point according to the discharge port position and the monitoring point position of the screened pollution source spectrum, the wind speed, the wind direction, the temperature, the pressure and the pollutant components.
Decomposing the number of main components in the monitoring data by applying a PCA data analysis method according to the monitoring data (pollutant concentration and component conditions); or an artificially set number of sources.
And calculating the contribution rate G of the corrected source spectrum data in the monitoring data by taking the number of the principal components, the monitoring data and the corrected source spectrum data as input and applying a PMF analysis method. Thereby tracing back the main contributor source of the contamination at the monitored location.
Scheme 2:
the required work comprises the steps of establishing a known source spectrum database (Si), wherein the known source spectrum database contains information including the pollutant composition proportion of a pollutant source discharge port and corresponding geographical position information; analyzing the wind speed and the wind direction at the source tracing moment, the position information of the monitoring points and the position information of the source spectrum database, and screening a discharge port of a pollution source which has great influence on the monitoring points; and converting the screened pollution source spectrum into a corrected source spectrum (Si') of the pollution source spectrum at the monitoring point according to the position of the discharge port and the monitoring point of the screened pollution source spectrum, the wind speed, the wind direction, the temperature, the pressure and the pollutant components.
And (3) taking the monitoring data and the corrected source spectrum data as input, calculating the contribution proportion of the corrected source spectrum data in the monitoring data to the monitoring data by applying a CMB analysis method, and tracing the main contribution source of the pollutants at the monitoring position.
The two tracing processes are more important steps of correcting source spectrum data. The emission point is at a certain distance from the actual monitoring point, and the concentration of each component in the source spectrum data has certain attenuation along with the increase of the distance, so the proportion of each component in the source spectrum data cannot be directly used for reflecting the proportion of each component after the source spectrum is transmitted to the monitoring point. And the data analysis result of the monitoring point and the spectral data of the emission point are directly analyzed, so that the tracing result is greatly influenced.
The source spectrum data is corrected, and firstly, according to objective factors of a pollution source spectrum, such as a discharge port position, a monitoring point position, and information of wind speed, wind direction, temperature, pressure, pollutant components and the like, a pollution source contributing to the monitoring point is screened out; and converting the source spectrum (Si) of the pollution source into a corrected source spectrum (Si ') of the pollution source at the monitoring point position or converting Sj into Sj' according to objective factors of the pollution source spectrum, such as air speed, wind direction, temperature, pressure, pollutant components, geographical position of the source spectrum and the like of the discharging position, geographical position information of the monitoring point and a diffusion model.
Correcting the relation between the source spectrum and the source spectrum data as
Si' = f (Si); alternatively, sj' = f (Sj)
The modified conversion function (f) represents a conversion relationship from the source spectrum data in the source spectrum database to the modified source spectrum data in the modified source spectrum database, and the modified conversion function includes at least one modification coefficient η.
Because factors such as atmospheric transportation and diffusion, photochemical reaction and the like have different influences on each component, the proportion and the absolute concentration of each component in a source spectrum are different after reaching a monitoring point from an emission point. Therefore, to better correct for the contamination source spectrum, a time span (duration) is introduced, which in this patent represents the time it takes for the source spectrum contamination to drift to the point of monitoring. The time distance is related to the distance from the pollutant source to the monitoring point and the pollutant diffusion speed, and the time distance is calculated in the following way,
time distance = distance/diffusion speed
The concentration at a certain time can be expressed by the following formula:
ci concentration of substance i (. Mu.g/m),
qi is the discharge rate of substance i (. Mu.g/m 2s 1),
h (t), a mixed height layer (m) at time t,
ri the decay rate of substance i (. Mu.g/m 3 s 1),
vd, i the dry/wet deposition rate (m/s 1) of substance i,
c0 i background concentration of substance i ((μ g/m 3)),
τ γ atmospheric residence time(s) of the zone,
ca i the concentration of substance i above the boundary layer (. Mu.g/m 3).
The diffusion speed is the result of the combination of transportation and diffusion, namely the result of the combined effects of physical transportation, gradient transportation, turbulent diffusion and the like. Physical transport can be expressed in terms of the component of wind speed on the source-to-monitor line, gradient transport and turbulent diffusion. The diffusion speed is related to the pollutant composition, wind direction, wind speed, diffusion conditions (temperature, pressure). The diffusion speed is the component of the wind speed on the connecting line of the source and the monitoring point, and is superposed with the Gaussian diffusion speed of the pollutants.
And introducing a correction coefficient on the basis of the time interval, wherein the material correction coefficient is related to the time interval and the objective condition at that time, and the correction coefficient is set according to the meteorological condition, the terrain, the underlying surface and the self property of the pollutant component. The correction coefficient is influenced by meteorological conditions such as wind speed and direction, temperature, illumination intensity and the like. Obstacles, terrain, etc. between the source and the monitoring point may also affect the correction factor.
The correction factor can be obtained by tracing, in addition to theoretical calculation. By adding the tracer substance into a certain pollution source discharge port, the correction coefficient is obtained by monitoring the attenuation degree of the tracer substance during monitoring. Alternative tracer materials are isotopes, VOCs that are easily monitored but are not present in the region, etc.
And (3) correcting the source spectrum data by adding a tracer substance: 1. a tracer substance is artificially added at a certain discharge source port and is released outwards at a stable concentration flow. 2. The concentration of the tracer substance is monitored at the monitoring point. 3. And comparing the concentration of the tracer substance of the monitoring point with the known concentration to obtain a correction coefficient. 4. And correcting the spectrogram of the source spectrum at the monitoring point through the correction coefficient. 5. The characteristics of other substances can be superposed on the basis of the correction coefficient of the tracer substance to obtain the correction coefficient of other specific substances. Alternative tracer materials are isotopes, VOCs that are easily monitored but are not present in the region, etc.
The correction coefficient may also be obtained by an empirical method, which obtains the correction coefficient experimentally. The correction coefficients of different substances at different distances are measured in advance through a large number of experiments.
The source spectral data was corrected by a number of experiments: firstly, under the condition of no wind, setting a distance. A contaminating substance is released at a constant concentration from the beginning of the distance and is monitored at the end of the distance. The correction factor can be obtained under the windless condition at the set distance by comparing the monitored concentration with the released concentration. And recording the wind speed and the wind direction under the windy condition, and constantly releasing a pollutant, wherein the ratio of the value measured from the tail end to the release concentration is the correction coefficient under the wind speed, the wind direction and the distance condition. By changing different wind speed, wind direction, distance, temperature and the like, a group of correction coefficient tables of a substance is obtained.
The correction coefficient under a certain condition of wind speed, wind direction, distance, temperature, etc. can be expressed by the following formula:
eta: the correction factor is a function of the number of pixels,
c i : the concentration of tracer substance i measured at a distance from the end (. Mu.g/m),
c i’ : the released concentration of tracer substance i (. Mu.g/m).
And (3) establishing a model method to correct the source spectrum data: 1. firstly, establishing a diffusion model, and establishing a three-dimensional space rectangular coordinate by a mathematical modeling method; 2. factors that affect the diffusion of volatile organics are determined, including weather conditions, terrain, underlying surface, nature of the contaminant components themselves. 3. Simplifying the basic form of the Gaussian model; 4. and establishing a volatile organic compound diffusion model in a small area range. 5. On the basis of a diffusion model, a secondary reaction of organic pollutants is added, namely the loss of VOCs active species is considered.
And (3) converting the VOCs data in the source spectrum library into the data of the monitoring points by using the following formula:
[VOC i ] t ＝[voc i ] o ×exp(-k i [OH]Δt)
[VOC i ] o ：VOC i observed values/values at monitoring points of the volume fraction;
[VOC i ] t ：VOC i an initial value of volume fraction;
b, C: primary hydrocarbons HCB and HCC exhausted from the same pollution source;
k i ：VOC i the OH radical reaction rate constant of (a);
k B : 0H of HCB fromFrom the radical reaction rate constant;
k C : OH radical reaction rate constant of HCC;
[ OH ]: volume fraction of OH radicals;
Δ t: reaction time;
Drawings
FIG. 1 is a flow chart of tracing a source using PCA and PMF methods;
FIG. 2 is a flow chart of tracing using the CMB method;
FIG. 3 is a schematic diagram showing the influence of wind direction on the concentration of a pollution source discharge port and a monitoring point;
FIG. 4 is a schematic view of the effect of multiple sources of pollution on a monitoring site under windy conditions;
FIG. 5 is a schematic illustration of the effect of two sources on a monitoring point;
FIG. 6 is a view of a wind direction vector decomposition of a single source on a monitoring point in case of wind;
FIG. 7 is a schematic diagram illustrating the determination of a source emission count based on a principal component load value;
FIG. 8 is a schematic diagram of the result of PMF operation;
FIG. 9 is a schematic diagram of the source contribution of TVOCs;
FIG. 10 is a schematic representation of benzene source contribution;
Detailed Description
Treatment of the recipient sample:
n samples (i.e., data collected at different collection times) each having p variables (i.e., p constituent materials) form an n × p order data matrix.
(1) Sample temporal resolution: the samples used are 1 minute averages. The sample size (collecting point number) is at least 5 times of the number of the monitoring factors, and the number of the samples is more than 80.
(2) Monitoring factors: PAMS, TO14 and organosulfur (36 mass TO charge ratios) with mass TO charge ratios within 40 TO 200 plus some common semi-quantitative substances (22 mass TO charge ratios), 58 in total, are all variables. Then, depending on the substance detected in the sample, it is required that the amount of the substance detected is more than 60% of the total sample amount (i.e. the detection rate is more than 60%, preferably this value is designed to be variable), otherwise this variable needs to be eliminated.
(3) The concentration of the screened substance is lower than the detection limit and is replaced by the detection limit.
(3) The concentration (. Mu.g/m 3) was used as an operation.
And (3) processing of a source spectrum sample:
the retention mass-to-charge ratio is 40-200, the concentration value is lower than the detection limit, and the detection limit is used instead. And finally, selecting variables the same as the receptor when the variables need to be compared with the result calculated by the receptor model, and then performing correlation comparison.
Receptor sample data matrix sourcing number:
the calculation is performed by the method of calculating the number of principal components in the principal component analysis.
(1) Firstly, a correlation coefficient matrix is calculated
rij (i, j =1,2, \ 8230;, p) is the correlation coefficient between the original variable xi and xj, and rij = rji and is calculated by the formula
(2) Computing eigenvalues and eigenvectors
Solving the characteristic equation λ I-R =0, finding characteristic values by the Jacobi method (Jacobi), and arranging λ in order of magnitude 1 ≥λ 2 ≥…≥λ p ≥0；
(3) Calculating principal component contribution rate and accumulated contribution rate (not calculating, only for reference of the number of emission sources screened later)
Contribution rate:
cumulative contribution rate:
generally, a characteristic value, lambda, with the accumulated contribution rate of 85% -95% is taken 1 ，λ 2 ，…，λ m The corresponding 1 st, 2 nd, \8230th, m (m is less than or equal to p) th main components.
(4) Calculating principal component loadings
Selecting the standard of the number of the emission sources: the first is the number Na obtained by extracting the characteristic value which is greater than 1; the second is with reference to principal component loadings, where the loading values in a principal component range from-1 to1, and a source is identified if the loading values in a principal component have more than 1 value greater than 0.5 or less than-0.5, and two sources are identified if the loading values in a principal component have more than 1 value greater than 0.5 and less than-0.5. The remaining principal components in the range of-0.5 to 0.5 are classified as a source. The sum of the number of sources contained in the principal component is the number of emission sources, see fig. 7.
The PMF method determines the source contribution pollution source contribution value and the pollution source component spectrum:
the idea of PMF (orthogonal Matrix Factorization) is as follows: firstly, the error of each chemical component in the atmosphere is calculated by using weight, and then the main pollution source and the contribution rate of the VOCs are determined by using a least square conjugate gradient method.
Where X is a matrix of n X p, n is the number of samples, and p is the chemical composition data, then the matrix X can be decomposed into a matrix G and a matrix F, where G is a matrix of emission source contributions from n X m VOCs, F is a matrix of pollution source composition spectra from m X p, and m is the number of primary pollution sources. Defining:
X＝GF+E
e is a residual matrix, representing the difference existing between X and GF.
The objective of the PMF analysis is to minimize Q, which is defined as:
I＝1，2，.......，n；j＝1，2，……，p；k＝1,2，……，m。
wherein S is the standard deviation of X; the elements of the X, G, F and E matrices, respectively.
Under the constraint condition that gik is more than or equal to 0 and fkj is more than or equal to 0, the contribution value G (relative value) of the pollution source and the component spectrum F (relative concentration value of chemical components) of the pollution source can be simultaneously determined by solving Q through an iterative minimization algorithm.
Optimizing the operation result: in practice, the minimum value of Q is found by running the program 100 times, and the value of the residual matrix E is observed to be as small as possible (-3 to 3), so as to ensure that the simulation result and the observation result have a better correlation, the PMF operation result refers to fig. 8, the tvocs source refers to fig. 9, and the benzene contribution source refers to fig. 10.
And (3) comparing with a source spectrum:
and comparing with a source spectrum, mainly performing Correlation analysis, namely performing Correlation analysis on the calculated pollution source component spectrum and the source spectrum respectively, wherein Pearson's Correlation is mainly used at present (a result is referred to as an accessory 4). Subsequent analysis of Kendall's tau-b correlation may be combined.
The results of Pearson correlation analysis were:
and (5) respectively replacing the Factor with the corresponding discharge point positions to obtain the final result.
Claims (15)
1. A tracing method for VOCs pollution comprises the following steps:
1) Building a known source spectrum database (Si): the source spectrum data in the known source spectrum database comprises the pollutant composition proportion of each known pollution source discharge port and the geographical position information of the discharge port;
2) Monitoring multiple groups of atmospheric VOCs data: monitoring the concentration and component conditions of pollutants in the atmosphere by a monitoring instrument to obtain monitoring data; the source number p can be obtained by calculating the data of a plurality of groups of atmospheric VOCs monitored by applying a factor analysis method or the source number p is set manually;
3) Screening a database of known source spectrums: screening source spectrum data by combining wind speed and wind direction in a tracing period, position information of monitoring points and geographical position information of discharge ports in a source spectrum database, screening discharge ports of pollution sources which have significant influence on the positions of the monitoring points, and removing discharge ports of the pollution sources which have no or little influence on the positions of the monitoring points; obtaining a source spectrum database (Sj) after screening;
4) Carrying out correction conversion on the screened source spectrum database (Sj) to obtain a corrected source spectrum database (Sj'): factors related to the correction conversion function (f) comprise the position of a monitoring point during sampling, wind speed, wind direction, temperature, pressure and pollutant components;
5) Analysis using PMF method: based on the source number p and the monitoring data, obtaining a pollution source component spectrum matrix (F) and the contribution ratio of each pollution source component spectrum (Fn) to the monitoring point by applying a PMF analysis method;
6) Carrying out component characteristic comparison and correlation comparison on the pollution source component spectrum (F) and each source spectrum data in the corrected source spectrum database (Sj'); and further obtaining the contribution ratio of each known pollution source discharge port at the monitoring point in the known source spectrum database.
2. A tracing method for VOCs pollution comprises the following steps:
1) Building a known source spectrum database (Si): the source spectrum data in the known source spectrum database comprises the pollutant composition proportion of each known pollution source discharge port and the geographic position information of the discharge port;
2) Monitoring multiple groups of atmospheric VOCs data: monitoring the concentration and component conditions of pollutants in the atmosphere by a monitoring instrument to obtain monitoring data; the source number p can be obtained by calculating the data of a plurality of groups of atmospheric VOCs monitored by applying a factor analysis method or the source number p is set manually;
3) Carrying out correction conversion on a known source spectrum database (Si) to obtain a corrected source spectrum database (Si'): factors related to the correction conversion function (f) comprise a monitoring point position during sampling, wind speed, wind direction, temperature, pressure and pollutant components;
4) Analysis using PMF method: based on the source number p and the monitoring data, obtaining a pollution source component spectrum matrix (F) and the contribution ratio of each pollution source component spectrum (Fn) to the monitoring point by applying a PMF analysis method;
5) Carrying out component characteristic comparison and correlation comparison on the pollution source component spectrum (F) and each source spectrum data in the corrected source spectrum database (Si'); and then the contribution proportion of each known pollution source discharge port in the known source spectrum database at the monitoring point is obtained.
3. A tracing method for VOCs pollution comprises the following steps:
1) Building a known source spectrum database (Si): the source spectrum data in the known source spectrum database comprises the pollutant composition proportion of each known pollution source discharge port and the geographical position information of the discharge port;
2) Monitoring multiple groups of atmospheric VOCs data: monitoring the concentration and component conditions of pollutants in the atmosphere by a monitoring instrument to obtain monitoring data; the source number p can be obtained by calculating the data of a plurality of groups of atmospheric VOCs monitored by applying a factor analysis method or the source number p is set manually;
3) Carrying out correction conversion on a known source spectrum database (Si) to obtain a corrected source spectrum database (Si'): factors related to the correction conversion function (f) comprise a monitoring point position during sampling, wind speed, wind direction, temperature, pressure and pollutant components;
4) Screening the modified source spectrum database (Si'): eliminating source spectrum data which have no influence or little influence on the position of the monitoring point; obtaining a screened correction source spectrum database (Sj');
5) Analysis using PMF method: based on the source number p and the monitoring data, obtaining a pollution source component spectrum matrix (F) and the contribution ratio of each pollution source component spectrum (Fn) to the monitoring point by applying a PMF analysis method;
6) Carrying out component characteristic comparison and correlation comparison on the pollution source component spectrum (F) and each source spectrum data in the corrected source spectrum database (Sj'); and further obtaining the contribution ratio of each known pollution source discharge port at the monitoring point in the known source spectrum database.
4. A tracing method for VOCs pollution comprises the following steps:
1) Building a known source spectrum database (Si): the source spectrum data in the known source spectrum database comprises the pollutant composition proportion of each known pollution source discharge port and the geographic position information of the discharge port;
2) Monitoring multiple groups of atmospheric VOCs data: monitoring the concentration and component conditions of pollutants in the atmosphere by a monitoring instrument to obtain monitoring data;
3) Screening a database of known source spectrums: screening source spectrum data by combining wind speed and wind direction in a tracing period, position information of monitoring points and geographical position information of discharge ports in a source spectrum database, screening discharge ports of pollution sources which have significant influence on the positions of the monitoring points, and removing discharge ports of the pollution sources which have no or little influence on the positions of the monitoring points; obtaining a source spectrum database (Sj) after screening;
4) Carrying out correction conversion on the screened source spectrum database (Sj) to obtain a corrected source spectrum database (Sj'): factors related to the correction conversion function (f) comprise the position of a monitoring point during sampling, wind speed, wind direction, temperature, pressure and pollutant components;
5) And (3) calculating the contribution proportion of the modified source spectrum at the monitoring point by applying a CMB analysis method: based on the monitoring data and the corrected source spectrum (Sj '), calculating the contribution proportion of the corrected source spectrum (Sj') at the monitoring point by applying a CMB analysis method;
6) And tracing the main contribution sources of the pollutants at the monitoring position according to the contribution proportion of each source spectrum data in the corrected source spectrum database (Sj') at the monitoring point.
5. A tracing method for VOCs pollution comprises the following steps:
1) Building a known source spectrum database (Si): the source spectrum data in the known source spectrum database comprises the pollutant composition proportion of each known pollution source discharge port and the geographic position information of the discharge port;
2) Monitoring multiple groups of atmospheric VOCs data: monitoring the concentration and component conditions of pollutants in the atmosphere by a monitoring instrument to obtain monitoring data;
3) Carrying out correction conversion on a known source spectrum database (Si) to obtain a corrected source spectrum database (Si'): factors related to the correction conversion function (f) comprise a monitoring point position during sampling, wind speed, wind direction, temperature, pressure and pollutant components;
4) And (3) calculating the contribution proportion of the modified source spectrum at the monitoring point by applying a CMB analysis method: calculating the contribution proportion of the corrected source spectrum (Si ') at the monitoring point by applying a CMB analysis method on the basis of the monitoring data and the corrected source spectrum (Si');
5) And tracing the main contribution sources of the pollutants at the monitoring position according to the contribution proportion of each source spectrum data in the corrected source spectrum database (Si') at the monitoring point.
6. A tracing method for VOCs pollution comprises the following steps:
1) Building a known source spectrum database (Si): the source spectrum data in the known source spectrum database comprises the pollutant composition proportion of each known pollution source discharge port and the geographical position information of the discharge port;
2) Monitoring multiple groups of atmospheric VOCs data: monitoring the concentration and component conditions of pollutants in the atmosphere by a monitoring instrument to obtain monitoring data;
3) Carrying out correction conversion on a known source spectrum database (Si) to obtain a corrected source spectrum database (Si'): factors related to the correction conversion function (f) comprise a monitoring point position during sampling, wind speed, wind direction, temperature, pressure and pollutant components;
4) Screening the corrected source spectrum database (Si'): eliminating source spectrum data which have no influence or little influence on the position of the monitoring point; obtaining a corrected source spectrum database (Sj')
5) And (3) calculating the contribution proportion of the modified source spectrum at the monitoring point by applying a CMB analysis method: based on the monitoring data and the corrected source spectrum (Sj '), calculating the contribution proportion of the corrected source spectrum (Sj') at the monitoring point by applying a CMB analysis method;
6) And tracing the main contribution sources of the pollutants at the monitoring position according to the contribution proportion of each source spectrum data in the corrected source spectrum database (Sj') at the monitoring point.
7. A tracing method for VOCs pollution comprises the following steps:
1) Building a known source spectrum database (Si): the source spectrum data in the known source spectrum database comprises the pollutant composition proportion of each known pollution source discharge port and the geographical position information of the discharge port;
2) Monitoring multiple groups of atmospheric VOCs data: monitoring the concentration and component conditions of pollutants in the atmosphere by a monitoring instrument to obtain monitoring data; the source number p can be obtained by calculating the data of a plurality of groups of atmospheric VOCs monitored by applying a factor analysis method or the source number p is set manually;
3) Screening a database of known source spectrums: the method comprises the steps of screening source spectrum data by combining wind speed and wind direction in a tracing period, position information of monitoring points and geographical position information of outlets in a source spectrum database, screening the outlets of pollution sources which have obvious influence on the monitoring points, and eliminating the outlets of the pollution sources which have no influence or little influence on the monitoring points; obtaining a source spectrum database (Sj) after screening;
4) Analysis using PMF method: based on the source number p and the monitoring data, obtaining a pollution source component spectrum matrix (F) and the contribution ratio of each pollution source component spectrum (Fn) to the monitoring point by applying a PMF analysis method;
5) Carrying out component characteristic comparison and correlation comparison on the pollution source component spectrum (F) and each source spectrum data in the screened source spectrum database (Sj); and further obtaining the contribution ratio of each known pollution source discharge port at the monitoring point in the known source spectrum database.
8. The method according to one of claims 1 to 6, wherein the modified transfer function (f) represents a transfer of source spectrum data in a source spectrum database to modified source spectrum data in a modified source spectrum database:
si' = f (Si); alternatively, sj' = f (Sj)
The correction conversion function comprises at least one correction coefficient eta.
9. The method of claim 8, wherein the correction factor is inversely proportional to a time distance, the time distance being time distance = distance/diffusion speed.
10. The method of claim 8, wherein the correction factor is inversely proportional to the photochemical reaction rate.
11. The method of claim 8, wherein the correction factor is calculated by,
η＝exp(-k i [OH]Δt)
wherein the content of the first and second substances,
b, C: primary hydrocarbons HCB and HCC exhausted from the same pollution source;
k i ：VOC i the OH radical reaction rate constant of (a);
k B : the OH radical reaction rate constant of HCB;
k C : OH radical reaction rate constant of HCC;
[ OH ]: volume fraction of OH radicals;
Δ t: reaction time;
12. The method of claim 8, wherein the correction factor is obtained empirically, the empirical method comprising the steps of,
1) Under the conditions of different wind directions, wind speeds, distances and humiture, a pollutant is constantly released from a discharge source, and the pollutant condition is monitored at the tail end of the distance;
2) Comparing the monitored concentrations and the release concentrations under the conditions of multiple groups of different wind directions, wind speeds, distances and humiture to obtain multiple groups of correction coefficients under the conditions of different wind directions, wind speeds, distances and humiture;
3) The wind direction, wind speed, distance, temperature and humidity conditions closest to the source tracing time are selected, and the correction coefficient under the conditions can be used as the correction coefficient of the source tracing time.
13. The method of any one of claims 1,3,4,6 or 7, wherein the screening step employs at least one of:
1) A dominant wind direction screening method;
2) A characteristic substance screening method;
3) Distance screening method: the monitoring point position and the geographical position of the discharge port in the source spectrum database can be screened out after a certain distance is exceeded; the remaining known source spectrum database is the source spectrum database after screening.
14. The method of claim 13, wherein the dominant wind direction screening method is: counting the occurrence frequency of each direction wind of the monitoring points in the acquisition process, representing the wind direction in different directions in a sixteen-compass azimuth coordinate system, representing the occurrence frequency by the distance from an original point, and then connecting the scattered points into a circular ring to form a wind-rose diagram, wherein the largest rose petal is the dominant wind direction of the monitoring points; and taking a connecting line between the main wind direction and the monitoring point as a center, and taking the known source spectrum data in a sector area with a certain included angle range as a source spectrum database after screening.
15. The method of claim 13, wherein the signature substance screening method is: if the source spectrum data is known not to contain the characteristic pollutant contained in the monitoring data, the source spectrum data can be screened out; if the known source spectrum data contain high-concentration characteristic pollutants which are not monitored at the monitoring point, the source spectrum data can be screened out; the remaining known source spectrum database is the source spectrum database after screening.
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